Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane

Wasalathanthri, Niluka D.; Guild, Curtis; Nizami, Quddus A.; Dissanayake, Shanka L.; He, Junkai; Kerns, Peter; Fee, Jared; Achola, Laura; Rathnayake, Dinithi; Weerakkody, Chandima; Suib, Steven L.; Nandi, Partha

doi:10.1039/C9RA04804A

Title: Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane

Abstract

Octahedral molecular sieve (OMS-2) refers to a one-dimensional 2 × 2 framework of octahedral manganese oxo units based on the cryptomelane-type framework. Herein, we describe a niobium (Nb) substituted mixed metal oxide of Nb and Mn where the cryptomelane-type framework is retained. These materials are hydrothermally synthesized from the reaction of potassium permanganate, manganese sulfate, and homogeneous niobium(V) precursors. Niobium incorporation up to 31 mol% can be achieved without destroying the one dimensional 2 × 2 framework. The yields of the materials vary between 70 and 90%. These materials are analyzed by powder XRD, BET isotherm, TEM, SEM, XRF, and XPS studies. The synthesized materials show promising activity in selective oxidation of methanol to dimethoxymethane (DMM) at 200 °C. Normalized activity correlations followed the trend 21% Nb-OMS-2 > 15% Nb-OMS-2 > 31% Nb-OMS-2 > 68% Nb-OMS-2 > K-OMS-2. A fluctuation in methanol conversion was observed around 125–150 °C in most samples, suggesting this to be a catalytically important temperature regime when forming active sites for DMM production.

Authors:

Wasalathanthri, Niluka D. ^[1]; Guild, Curtis ^[1]; Nizami, Quddus A. ^[2]; Dissanayake, Shanka L. ^[1]; He, Junkai ^[3]; Kerns, Peter ^[1]; Fee, Jared ^[1]; Achola, Laura ^[1]; Rathnayake, Dinithi ^[1]; Weerakkody, Chandima ^[1];

^[4]; Nandi, Partha ^[2]

Department of Chemistry, University of Connecticut, Storrs, USA
Corporate Strategic Research, ExxonMobil Research and Engineering Company, Annandale, USA
Institute of Material Science, University of Connecticut, Storrs, USA
Department of Chemistry, University of Connecticut, Storrs, USA, Institute of Material Science

Publication Date:: 2019-10-14

Research Org.:: Univ. of Connecticut, Storrs, CT (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

OSTI Identifier:: 1574081

Alternate Identifier(s):: OSTI ID: 1598224

Grant/Contract Number:: FG02-86ER13622

Resource Type:: Published Article

Journal Name:: RSC Advances

Additional Journal Information:: Journal Name: RSC Advances Journal Volume: 9 Journal Issue: 56; Journal ID: ISSN 2046-2069

Publisher:: Royal Society of Chemistry

Country of Publication:: United Kingdom

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Wasalathanthri, Niluka D., Guild, Curtis, Nizami, Quddus A., Dissanayake, Shanka L., He, Junkai, Kerns, Peter, Fee, Jared, Achola, Laura, Rathnayake, Dinithi, Weerakkody, Chandima, Suib, Steven L., and Nandi, Partha. Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane.  United Kingdom: N. p., 2019. 
Web.  doi:10.1039/C9RA04804A.

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                    Wasalathanthri, Niluka D., Guild, Curtis, Nizami, Quddus A., Dissanayake, Shanka L., He, Junkai, Kerns, Peter, Fee, Jared, Achola, Laura, Rathnayake, Dinithi, Weerakkody, Chandima, Suib, Steven L., & Nandi, Partha. Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane.  United Kingdom.  https://doi.org/10.1039/C9RA04804A

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                    Wasalathanthri, Niluka D., Guild, Curtis, Nizami, Quddus A., Dissanayake, Shanka L., He, Junkai, Kerns, Peter, Fee, Jared, Achola, Laura, Rathnayake, Dinithi, Weerakkody, Chandima, Suib, Steven L., and Nandi, Partha. Mon .  
"Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane".  United Kingdom.  https://doi.org/10.1039/C9RA04804A.

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@article{osti_1574081,

  title        = {Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane},

  author       = {Wasalathanthri, Niluka D. and Guild, Curtis and Nizami, Quddus A. and Dissanayake, Shanka L. and He, Junkai and Kerns, Peter and Fee, Jared and Achola, Laura and Rathnayake, Dinithi and Weerakkody, Chandima and Suib, Steven L. and Nandi, Partha},

  abstractNote = {Octahedral molecular sieve (OMS-2) refers to a one-dimensional 2 × 2 framework of octahedral manganese oxo units based on the cryptomelane-type framework. Herein, we describe a niobium (Nb) substituted mixed metal oxide of Nb and Mn where the cryptomelane-type framework is retained. These materials are hydrothermally synthesized from the reaction of potassium permanganate, manganese sulfate, and homogeneous niobium(V) precursors. Niobium incorporation up to 31 mol% can be achieved without destroying the one dimensional 2 × 2 framework. The yields of the materials vary between 70 and 90%. These materials are analyzed by powder XRD, BET isotherm, TEM, SEM, XRF, and XPS studies. The synthesized materials show promising activity in selective oxidation of methanol to dimethoxymethane (DMM) at 200 °C. Normalized activity correlations followed the trend 21% Nb-OMS-2 > 15% Nb-OMS-2 > 31% Nb-OMS-2 > 68% Nb-OMS-2 > K-OMS-2. A fluctuation in methanol conversion was observed around 125–150 °C in most samples, suggesting this to be a catalytically important temperature regime when forming active sites for DMM production.},

  doi          = {10.1039/C9RA04804A},

  journal      = {RSC Advances},

  number       = 56,

  volume       = 9,

  place        = {United Kingdom},

  year         = {2019},

  month        = {10}

}

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Title: Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane

Abstract

Citation Formats

Selective oxidation of methanol to dimethoxymethane under mild conditions over V2O5/TiO2 with enhanced surface acidity journal, January 2007

Manganese Oxide-catalyzed Additive- and Solvent-free Aerobic Oxidative Synthesis of Primary Amides from Primary Amines journal, June 2012

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Selective oxidation of methanol to dimethoxymethane over bifunctional VOx/TS-1 catalysts journal, January 2011

Manganese Oxide Octahedral Molecular Sieves (OMS-2) Multiple Framework Substitutions: A New Route to OMS-2 Particle Size and Morphology Control journal, November 2010

Study of the Partial Oxidation of Methanol to Formaldehyde on a Polycrystalline Ag Foil journal, June 2001

Characterization of the Fe-Doped Mixed-Valent Tunnel Structure Manganese Oxide KOMS-2 journal, October 2011

Mesoporous manganese oxides for NO2 assisted catalytic soot oxidation journal, February 2017

A decatungstate-type polyoxoniobate with centered manganese: [H2MnIVNb10O32]8− as a soluble tetramethylammonium salt journal, January 2013

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Practical methods for measuring the tortuosity of porous materials from binary or gray-tone tomographic reconstructions journal, August 2009

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